助剂对顺酐加氢制备γ-丁内酯催化剂页硅酸镍性能的影响
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摘要
采用蒸氨法制备含Mo、Ce、Zn助剂的页硅酸镍催化剂,考察助剂对催化剂催化顺酐加氢制备γ-丁内酯的影响。结合N2吸附-脱附、XRD、H2-TPR、NH3-TPD、TEM、XPS等表征和活性评价对催化剂的织构性质及其催化性能进行研究。结果表明,不同性质的助剂对催化剂结构及其催化性能具有显著影响。助剂Mo的掺杂,提高催化剂中镍物种的还原,增加催化剂表面金属Ni0的数目,在金属和酸性位协同催化下,促进催化剂催化顺酐C=O基加氢的能力,在反应温度160℃、氢气压力5 MPa、反应时间180 min条件下,γ-丁内酯产率可达21. 3%,是未掺杂催化剂催化活性的1. 5倍。助剂Zn和Ce的加入,降低催化剂酸性,进而降低其催化活性。
Effects of Mo,Ce and Zn promoters on nickel phyllosilicate( Ni-PS) catalyst prepared by ammonia distillation for hydrogenation of maleic anhydride to γ-butyrolactone were investigated. N2 adsorption-desorption,XRD,H2-TPR,NH3-TPD,TEM and XPS characterization techniques combined with activity tests were carried out to explore the physicochemical properties and catalytic performance of the catalysts. The results indicated that promoters had significantly influence on structure and catalytic activity of the catalysts. The doping of Mo enhanced the reduction degree of Ni and led to more metal Ni0 on the catalyst surface. Due to the synergistic effect between the surface Ni0 and acid sites,the doping of Mo remarkably improved the activity of Ni-Si catalyst for the hydrogenation of C=O group in maleic anhydride. At reaction temperature of 160 ℃,H2 pressure of 5 MPa an reaction time of 180 min,yield ofγ-butyrolactone was up to 21. 3%,which was about 1. 5 times than that of catalyst without doping. However,addition of Zn and Ce greatly reduced the acidity of the catalyst and then reduced catalytic activity.
Effects of Mo,Ce and Zn promoters on nickel phyllosilicate( Ni-PS) catalyst prepared by ammonia distillation for hydrogenation of maleic anhydride to γ-butyrolactone were investigated. N2 adsorption-desorption,XRD,H2-TPR,NH3-TPD,TEM and XPS characterization techniques combined with activity tests were carried out to explore the physicochemical properties and catalytic performance of the catalysts. The results indicated that promoters had significantly influence on structure and catalytic activity of the catalysts. The doping of Mo enhanced the reduction degree of Ni and led to more metal Ni0 on the catalyst surface. Due to the synergistic effect between the surface Ni0 and acid sites,the doping of Mo remarkably improved the activity of Ni-Si catalyst for the hydrogenation of C=O group in maleic anhydride. At reaction temperature of 160 ℃,H2 pressure of 5 MPa an reaction time of 180 min,yield ofγ-butyrolactone was up to 21. 3%,which was about 1. 5 times than that of catalyst without doping. However,addition of Zn and Ce greatly reduced the acidity of the catalyst and then reduced catalytic activity.
引文
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[25]Miller J B,Rankin S E,Ko E I. Strategies in controlling the homogeneity of zirconia-silica aerogels:effect of preparation on textural and catalytic properties[J]. Journal of Catalysis,1994,148:673-682.
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[27]Das S,Ashok J,Bian Z,et al. Silica-ceria sandwiched Ni core-shell catalyst for low temperature dry reforming of biogas:coke resistance and mechanistic insights[J].Applied Catalysis B:Environmental,2018,230:220-236.
[28]Zhao Xiaolan,Wang Yun,Wu Hanyu,et al. Insights into the effect of humic acid on Ni(II)sorption mechanism on illite:batch,XPS and EXAFS investigations[J]. Journal of Molecular Liquids,2017,248:1030-1038.
[29]Lehmann T,Wolff T,Hamel C,et al. Physico-chemical characterization of Ni/MCM-41 synthesized by a template ion exchange approach[J]. Microporous and Mesoporous Materials,2012,151:113-125.
[30]Kim K S,Winograd Nicholas. X-ray photoelectron spectroscopic studies of nickel-oxygen surfaces using oxygen and argon ion-bombardment[J]. Surface Science,1974,43:625-643.
[31]Li Ziwei,Jiang Bo,Wang Zhigang,et al. High carbon resistant Ni@Ni phyllosilicate@Si O2core shell hollow sphere catalysts for low temperature CH4dry reforming[J]. Journal of CO2Utilization,2018,27:238-246.
[32]Sawhill S J,Layman K A,Van W D R,et al. Thiophene hydrodesulfurization over nickel phosphide catalysts:effect of the precursor composition and support[J]. Journal of Catalysis,2005,231:300-313.
[2]Xu Youmin,Bi Yadong,Yin Xiaohong. Liquid phase hydrogenation of maleic anhydride over Ni catalysts:effect of support on the catalytic performance[J]. Advanced Materials Research,2014,1033-1034:57-60.
[3]Lan Jihong,Lin Jinchi,Chen Zhuqi,et al. Transformation of5-hydroxymethylfurfural(HMF)to maleic anhydride by aerobic oxidation with heteropolyacid catalysts[J]. ACS Catalysis,2015,5:2035-2041.
[4]Alonso-Fagundez N,Ojeda M,Mariscal R,et al. Gas phase oxidation of furfural to maleic anhydride on V2O5/γ-Al2O3catalysts:reaction conditions to slow down the deactivation[J]. Journal of Catalysis,2017,348:265-275.
[5]Regenhardt Silivina A,Meyer Camilo I,Garetto Teresita F,et al. Selective gas phase hydrogenation of maleic anhydride over Ni-supported catalysts:effect of support on the catalytic performance[J]. Applied Catalysis A:General,2012,449:81-87.
[6]Hong Unggi,Park Haiwoong,Lee Joongwon,et al. Hydrogenation of succinic acid toγ-butyrolactone(GBL)over ruthenium catalyst supported on surfactant-templated mesoporous carbon[J]. Journal of Industrial and Engineering Chemistry,2012,18:462-468.
[7]Yu Yang,Zhan Wangcheng,Guo Yun,et al. Gas-phase hydrogenation of maleic anhydride toγ-butyrolactone over Cu-Ce O2-Al2O3catalyst at atmospheric pressure:effects of the residual sodium and water in the catalyst precursor[J]. Journal of Molecular Catalysis A:Chemical,2014,395:392-397.
[8]Zhang Bin,Zhu Yulei,Ding Guoqiang,et al. Modification of the supported Cu/Si O2catalyst by alkaline earth metals in the selective conversion of 1,4-butanediol toγ-butyrolactone[J].Applied Catalysis A:General,2012,443-444:191-201.
[9]Yuan Hongjing,Zhang Chuanlei,Huo Weitao,et al. Selective hydrogenation of maleic anhydride over Pd/Al2O3catalysts prepared via colloid deposition[J]. Journal of Chemical Science,2014,126(1):141-145.
[10]Huo Weitao,Zhang Chunlei,Yuan Hongjing,et al. Vaporphase selective hydrogenation of maleic anhydride to succinic anhydride over Ni/Ti O2catalysts[J]. Journal of Industrial and Engineering Chemistry,2014,20(6):4140-4145.
[11]Huang Yangqiang,Ma Yao,Cheng Youwei,et al. Active ruthenium catalysts prepared by cacumen platycladi leaf extract for selective hydrogenation of maleic anhydride[J]. Applied Catalysis A:General,2015,495:124-130.
[12]Liao Xin,Zhang Yin,Hill Martyn,et al. Highly efficient Ni/Ce O2catalyst for the liquid phase hydrogenation of maleic anhydride[J]. Applied Catalysis A:General,2014,488:256-264.
[13]Liao Xin,Zhang Yin,Guo Junqiu,et al. The catalytic hydrogenation of maleic anhydride on Ce O2-δ-supported transition metal catalysts[J]. Catalysts,2017,7(9):272-287.
[14]徐爱军,梁二艳,王杰,等.络合浸渍法制备Ni/Zr O2催化剂及其催化顺酐液相加氢性能[J].工业催化,2018,26(2):28-32.Xu Aijun,Liang Eryan,Wang Jie,et al. Preparation of Ni/Zr O2catalysts for liquid hydrogenation of maleic anhydride by complex impregnation[J]. Industrial Catalysts,2018,26(2):28-32.
[15]Cui Jinglei,Tan Jingjing,Zhu Yulei,et al. Aqueous hydrogenation of levulinic acid to 1,4-pentanediol over Momodified Ru/activated carbon catalyst[J]. Chem Sus Chem,2018,11:1316-1320.
[16]Kong Xiao,Zhu Yifeng,Zheng Hongyan,et al. Ni nanoparticles inlaid nickel phyllosilicate as a metal-acid bifunctional catalyst for low-temperature hydrogenolysis reactions[J]. ACS Catalysis,2015,5(10):5914-5920.
[17]Wang Yue,Shen Yongli,Zhao Yujun,et al. Insight into the balancing effect of active Cu species for hydrogenation of carbon-oxygen bonds[J]. ACS Catalysis,2015,5(10):6200-6208.
[18]陶然,陈吉祥,张继炎.助剂对加氢催化剂Ni/Si O2结构和反应性能的影响[J].化学工业与工程,2005,22(3):175-178.Tao Ran,Chen Jixiang,Zhang Jiyan. Effects of promoters on structure and properties of Ni/Si O2catalysts for hydrogenation[J]. Chemical Industry and Engineering,2005,22(3):175-178.
[19]刘迎新,张继炎,陈吉祥,等.助剂对Ni/Si O2催化剂结构和间二硝基苯加氢性能的影响[J].石油学报(石油加工),2005,21(2):58-62.Liu Yingxin,Zhang Jiyan,Chen Jixiang,et al. Effect of promoters on physico-chemical propertis and catalytic performance of Ni/Si O2in m-dinitrobenzene hydrogenation[J]. Acta Petrolei Sinic(Petroleum Processing Section),2005,21(2):58-62.
[20]Maluf S S,Assaf E M. Ni catalysts with Mo promoter for methane steam reforming[J]. Fuel,2009,88:1547-1553.
[21]Gatti M N,Mizrahi M D,Ramallo-Lopez J M,et al.Improvement of the catalytic activity of Ni/Si O2-C by the modification of the support and Zn addition:bio-propylene glycol from glycerol[J]. Applied Catalysis A:General,2017,548:24-32.
[22]Zhang Chengxi,Yue Hairong,Huang Zhiqi,et al. Hydrogen production via steam reforming of ethanol on phyllosilicatederived Ni/Si O2:enhanced metal-support interaction and catalytic stability[J]. ACS Sustainable Chemistry&Engineering,2013,1(1):161-173.
[23]Clause O,Bonneviot L,Che M. Effect of the preparation method on the thermal stability of silica-supported nickel oxide as studied by EXAFS and TPR techniques[J]. Journal of Catalysis,1992,138:195-205.
[24]Sun Keqiang,Marceau Eric,Che Michel. Evolution of nickel speciation during preparation of Ni-Si O2catalysts:effect of the number of chelating ligands in[Ni(en)x(H2O)6-2x]2+precursor complexes[J]. Physical Chemistry Chemical Physics,2006,8:1731-1738.
[25]Miller J B,Rankin S E,Ko E I. Strategies in controlling the homogeneity of zirconia-silica aerogels:effect of preparation on textural and catalytic properties[J]. Journal of Catalysis,1994,148:673-682.
[26]Anderson J A,Fergusson C,Rodriguez-Ramos I,et al.Influence of Si/Zr ratio on the formation of surface acidity in silica-zirconia aerogels[J]. Journal of Catalysis,2000,192:344-354.
[27]Das S,Ashok J,Bian Z,et al. Silica-ceria sandwiched Ni core-shell catalyst for low temperature dry reforming of biogas:coke resistance and mechanistic insights[J].Applied Catalysis B:Environmental,2018,230:220-236.
[28]Zhao Xiaolan,Wang Yun,Wu Hanyu,et al. Insights into the effect of humic acid on Ni(II)sorption mechanism on illite:batch,XPS and EXAFS investigations[J]. Journal of Molecular Liquids,2017,248:1030-1038.
[29]Lehmann T,Wolff T,Hamel C,et al. Physico-chemical characterization of Ni/MCM-41 synthesized by a template ion exchange approach[J]. Microporous and Mesoporous Materials,2012,151:113-125.
[30]Kim K S,Winograd Nicholas. X-ray photoelectron spectroscopic studies of nickel-oxygen surfaces using oxygen and argon ion-bombardment[J]. Surface Science,1974,43:625-643.
[31]Li Ziwei,Jiang Bo,Wang Zhigang,et al. High carbon resistant Ni@Ni phyllosilicate@Si O2core shell hollow sphere catalysts for low temperature CH4dry reforming[J]. Journal of CO2Utilization,2018,27:238-246.
[32]Sawhill S J,Layman K A,Van W D R,et al. Thiophene hydrodesulfurization over nickel phosphide catalysts:effect of the precursor composition and support[J]. Journal of Catalysis,2005,231:300-313.
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